Among the nanomedecine challenges, engineering nanomaterials able to combine imaging and multi-therapies is hugely needed to address issues of a personalized treatment. In that context, a novel class of drug releasing and remotely activated nanocomposites based on carbon-based materials coated with mesoporous silica and loaded with an outstanding level of the anti-tumoral drug doxorubicin (DOX) has been designed. Such nanocomposites are shown able thus to combine drug delivery, phototherapy and imaging, thanks to the carbon based materials. First, carbon nanotubes (CNTs) and graphene sheets (called "few layer graphene" FLGs) are processed to afford a distribution size that is more suitable for nanomedicine applications. Then, the controlled coating of mesoporous silica (MS) shell having a thickness tailored with the sol-gel parameters (amount of precursor, sol-gel time) around the sliced CNTs and exfoliated FLGs are reported. Furthermore, the drug loading in such mesoporous nanocomposites is investigated in full and the surface modification with an aminopropyltriethoxysilane (APTS) coating leading to a controlled polysiloxane layer provides an ultra-high payload of DOX (up to 3 folds the mass of the composites). Such new

One key challenge in the fields of nanomedicine and tissue engineering is the design of theranostic nanoplatforms able to monitor their therapeutic effect by imaging. Among current developed nano-objects, carbon nanotubes (CNTs) were found suitable to combine imaging, photothermal therapy, and to be loaded with hydrophobic drugs. However, a main problem is their resulting low hydrophilicity. To face this problem, an innovative method is developed here, which consists in loading the surface of carbon nanotubes (CNTs) with drugs followed by a protein coating around them. The originality of this method relies on first covering CNTs with a sacrificial template mesoporous silica (MS) shell grafted with isobutyramide (IBAM) binders on which a protein nanofilm is strongly adhered through IBAM-mediated physical cross-linking. This concept is first demonstrated without drugs, and is further improved with the suitable loading of hydrophobic drugs, curcumin (CUR) and camptothecin (CPT), which are retained between the CNTs and human serum albumin (HSA) layer. Such novel nanocomposites with favorable photothermal properties are very promising for theranostic systems, drug delivery, and phototherapy applications.