Development of covalent organic frameworks (COFs) with circularly polarized luminescence (CPL) is still challenging. Here we first reported ultrathin COFs nanosheets (NS) based CPL materials using a chiral induced-synthesis strategy. Chiral amines served as chiral inducers to give COF TpBpy with chirality and participated in the modification of TpBpy, inhibiting the fluorescence quenching caused by π-π stacking to form ultrathin luminescent chiral COFs (chirCOFs) NS. The obtained chirCOFs -/-TpBpy NS had strong chirality and intense red CPL property with a || of ∼0.02. Afterward, the carboxyl containing green and blue fluorescent dye molecules were postmodified onto the chirCOFs NS (chirCOFs/Dyes) to achieve color-adjustable CPL. Due to the chirality and energy transfer between chirCOFs and dye groups, the obtained chirCOFs/Dyes showed strong chirality and increased and tunable photoluminescence, exhibiting excellent, tunable, and amplified CPL performance with a maximum || of ∼0.1, which was ∼5 times stronger than that of as-prepared chirCOFs NS. Moreover, the corresponding chirCOFs NS were dispersed into a polydimethylsiloxane (PDMS) matrix to form wafer size, highly transparent, and flexible COFs/PDMS films for practical CPL application. This study opens a new strategy to prepare ultrathin chirCOFs NS with strong and tunable CPL by chiral induction and provides a new approach for the preparation of transparent, large size, and flexible COFs composite films in chiral optical applications.