in bioimaging application. On the other hand, great research interest has been focused on pure organic persistent RTP materials in recent years because they exhibit superior environmental friendliness, low cost, good biocompatibility, impressive stability, and easy modification. To meet the requirements of intravital bioimaging, the development of effective and ultralong pure organic RTP materials is desirable, where the promotion of intersystem crossing (ISC) and inhibition of nonradiative decay play key roles.Two approaches are summarized in accordance with the first-order perturbation theory and the Marcus semiclassical approach: [5] One approach is to increase the spin-orbital coupling (SOC) and promote the ISC processes by introducing heteroatoms with lone pair electrons, [6] heavy atoms, [7] or carbonyls; [8] the other approach is to suppress the nonradiative relaxation pathways and subsequently stabilize the triplet excitons in a stiff environment by forming crystals, [9] polymer assistance, [10] H-aggregation, [11] host-guest combination, [12] etc. With unremitting efforts, impressive advancements have been made in the past decade. For instance, Kim and co-workers developed an efficient pure organic RTP system to realize materials with bright RTP and a quantum yield (Φ) of 55% by forming cocrystals with a similar halogen-bonding motif. [13] Moreover, Huang and co-workers developed a new strategy for prolonging the phosphorescence lifetime by using d-pπ bonds to regulate the excited-state electronic configuration of pure organic Pure organic persistent room temperature phosphorescence (RTP) materials have attracted wide attention owing to their great potential in various applications, particularly in bioimaging. However, it is still a challenge to manufacture organic RTP materials possessing quite high efficiency and long lifetime, owing to the high requirements for triplet excitons. In this study, a series of keto derivatives with efficient RTP in crystals are developed through the regulation of molecular aggregation states by simple alkyl groups, resulting in impressive luminescence performance with a longer lifetime and higher efficiency of up to 868 ms and 51.59%, respectively. All the alkyl-substituted derivatives exhibit bright RTP intensities after heavy grinding with a pestle, indicating their robust RTP features, which are suitable for many fields. Encouraged by the excellent RTP performance of these luminogens in the crystalline state, successful orthotopic lung tumor imaging with a high signal-to-background ratio (SBR) of 65 is demonstrated in this study to provide the promise of pure organic RTP materials for disease diagnosis, which hold the advantages of low autofluorescence interference and high signal-to-background ratio.