Stimulating and harnessing circularly polarized luminescence (CPL) is not only a sine qua non for fundamentally unveiling chirogenesis in physical chemistry, and also a pivotal prerequisite for implementation of such phenomenon in area of chiral optoelectronics and theranostics. Herein, red-emissive carbonized polymer dots (CPDs)-based helical structures were synthesized in this work via biomolecule-tailored organic-inorganic co-assembly strategy. The surface states related chirality exhibited enhanced circular dichroism (CD) and CPL activities with anisotropic factors as high as gCD,max=5.4×10-3 and glum,max=1.5×10-2 respectively. The obtained CPL signals can be further manipulated with an excitation-dependent manner indicating a synergistic-competition phenomenon is existed between configurational chirality and intermolecular energy-transfer dynamics, which is further supported by simulations based on density function theory (DFT). Such tunable CPL behaviors triggers revolutionary designs and applications of these chiral CPDs into the realm of chirality-related biological issues and next generation chiral optoelectronics.