Cell‐membrane‐coated nanoparticles (CCNPs) that integrate the biophysiological advantages of cell membranes with the multifunctionalities of synthetic materials hold great promise in cancer immunotherapy. However, strategies have yet to be revealed to further improve their immunotherapeutic efficacy. Herein, a polymer multicellular nanoengager (SPNE) for synergistic second‐near‐infrared‐window (NIR‐II) photothermal immunotherapy is reported. The nanoengager consists of an NIR‐II absorbing polymer as the photothermal core, which is camouflaged with fused membranes derived from immunologically engineered tumor cells and dendritic cells (DCs) as the cancer vaccine shell. In association with the high accumulation in lymph nodes and tumors, the multicellular engagement ability of the SPNE enables effective cross‐interactions among tumor cells, DCs, and T cells, leading to augmented T cell activation relative to bare or tumor‐cell‐coated nanoparticles. Upon deep‐tissue penetrating NIR‐II photoirradiation, SPNE eradicates the tumor and induces immunogenic cell death, further eliciting anti‐tumor T cell immunity. Such a synergistic photothermal immunotherapeutic effect eventually inhibits tumor growth, prevents metastasis and procures immunological memory. Thus, this study presents a general cell‐membrane‐coating approach to develop photo‐immunotherapeutic agents for cancer therapy.

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Zein and hyaluronic acid (HA) composite nanoparticles were self-assembly fabricated using antisolvent coprecipitation (ASCP) method to deliver quercetagetin (Que). FTIR, CD, and FS results revealed that electrostatic attraction, hydrogen bonding, and hydrophobic effect were the dominant driving forces among zein, Que, and HA. With the increasing of HA level, the morphological structure of zein-Que-HA complex was changed from nanoparticle (from 100:5:5 to 100:5:20) to microgel (from 100:5:25 to 100:5:30). The encapsulation efficiency of Que has significantly increased from 55.66% (zein-Que, 100:5) to 93.22% (zein-Que-HA, 100:5:20), and Que in the zein-Que-HA composite nanoparticles exhibited obviously enhanced photochemical, thermal, and physical stability. After 8 months of storage (4 °C), the retention rate of Que also up to 77.93%. These findings interpreted that zein-HA composite nanoparticle would be an efficient delivery system for encapsulating and protecting bioactive compounds.

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The utilization of layer-by-layer composite nanoparticles fabricated from zein and hyaluronic acid (HA) for the codelivery of curcumin and quercetagetin was investigated. A combination of hydrophobic effects and hydrogen bonding was responsible for the interaction of zein with both curcumin and quercetagetin inside the nanoparticles. Electrostatic attraction and hydrogen bonding were mainly responsible for the layer-by-layer deposition of hyaluronic acid on the surfaces of the nanoparticles. The secondary structure of zein was altered by the presence of the two nutraceuticals and HA. The optimized nanoparticle formulation contained relatively small particles (d = 231.2 nm) that were anionic (ζ = −30.5 mV). The entrapment efficiency and loading capacity were 69.8 and 2.5% for curcumin and 90.3 and 3.5% for quercetagetin, respectively. Interestingly, the morphology of the nanoparticles depended on their composition. In particular, they changed from coated nanoparticles to nanoparticle-filled microgels as the level of HA increased. The nanoparticles were effective at reducing light and thermal degradation of the two encapsulated nutraceuticals and remained physically stable throughout 6 months of long-term storage. In addition, the nanoparticles were shown to slowly release the nutraceuticals under simulated gastrointestinal tract conditions, which may help improve their oral bioavailability. In summary, we have shown that layer-by-layer composite nanoparticles based on zein and HA are an effective codelivery system for two bioactive compounds.

Curcumin and piperine are natural nutraceuticals that exhibit synergistic biological activities, but have different polarities, which can make their encapsulation within a single delivery system challenging. In this study, the two bioactive components were encapsulated within core–shell nanoparticles formed by a combination of antisolvent precipitation and layer-by-layer deposition. Initially, strongly hydrophobic curcumin (log P = 4.12) was embedded in the hydrophobic core of zein-hyaluronic acid nanoparticles using the antisolvent precipitation method. Then, the weakly hydrophobic piperine (log P = 2.78) was adsorbed to the outer biopolymer shell of these nanoparticles. Finally, the nutraceutical-loaded particles were coated with a layer of chitosan by the electrostatic deposition method. The surface charge and coating thickness depended on the number of adsorbed layers and the nature of the outer layer, being negative for hyaluronic acid and positive for chitosan. Low-, medium-, and high-molecular weight chitosan were utilized to modify the surface properties. Chitosan with a low-molecular weight was selected to fabricate the core–shell nanoparticles because it produced small highly charged cationic particles (d = 599 nm; ζ = +38.1 mV). The encapsulation efficiency and loading capacities were 90.4 and 5.7% for curcumin, and 86.4 and 5.4% for piperine, respectively. The core–shell nanoparticles protected the nutraceuticals from chemical degradation during light exposure, thermal processing, and storage for 2 months. Moreover, the nanoparticles were able to control the release of the bioactive components in simulated gastrointestinal conditions. Our results should facilitate the development of more effective nanodelivery systems for nutraceuticals that exhibit synergistic activities, but have different molecular characteristics.

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