Flexible piezoelectric ceramic composites (FPCCs) hold promising applications in fields such as flexible sensing and energy harvesting. However, the previous methods are difficult to achieve high-precision preparation of the FPCCs with complex structures, as well as the synergistic enhancement of piezoelectric performance and flexibility. In this study, by configuring a flexible resin matrix and employing a surface functionalization treatment on the piezoelectric ceramic particles, the flexibility and piezoelectric performance of the FPCCs are synergistically improved. Moreover, the addition of a light absorber, TiO2, significantly improves the 3D printing precision. The mechanical properties, piezoelectric performance, and printing precision of the FPCCs are analyzed. It is found that the printing error is less than 2 μm, the tensile fracture strength is 4.07 MPa, the elongation at break is 350 %, and the piezoelectric constant d33 can reach 7.7 pC/N. In addition, the cyclic loading tests show that FPCCs with high-precision 3D complex microstructure have good recovery performance. This study not only enriches the formulation of FPCCs slurry for 3D printing, but also provides a research foundation for the multifunctional applications.