Organic luminescent materials are indispensable in optoelectronic displays and solid‐state luminescence applications. Compared with single‐component, multi‐component crystalline materials can improve optoelectronic characteristics. This work forms a series of full‐spectrum tunable luminescent charge‐transfer (CT) cocrystals ranging from 400 to 800 nm through intermolecular collaborative self‐assembly. What is even more interesting is that o‐TCP‐Cor(x)‐Pe(1−x), p‐TCP‐Cor(x)‐Pe(1−x), and o‐TCP‐AN(x)‐TP(1−x) alloys are prepared based on cocrystals by doping strategies, which correspondingly achieve the stepless color change from blue (CIE [0.22, 0.44]) to green (CIE [0.16, 0.14]), from green (CIE [0.27, 0.56]) to orange (CIE [0.58, 0.42]), from yellow (CIE [0.40, 0.57]) to red (CIE [0.65, 0.35]). The work provides an efficient method for precisely synthesizing new luminescent organic semiconductor materials and lays a solid foundation for developing advanced organic solid‐state displays.