Motivated by the need of piezoelectric ceramics with enhanced piezoelectric properties, we investigated the effects of Sr addition on the structural, dielectric and piezoelectric properties of PMN-PT ceramics. The synthesis of (1-x)[(Pb1−ySry)(Mg1/3Nb2/3)O3]-x(Pb1−ySryTiO3) (PsMN–PsT) (y: 0 − 0.10, x: 0.35 – 0.40) ceramics was carried out by the colloidal coating method to distribute Sr uniformly in PMN and PT respectively. When x=0.35, it was found that y=0.02 gave the optimal piezoelectric properties. Furthermore, by keeping y=0.02 and varying x, it was found that x=0.37 gave even better piezoelectric properties with the optimal piezoelectric strain coefficient d33 (630 pC/N), piezoelectric coupling factor kp (0.52), dielectric constant εr (4000), and Curie temperature Tc (210°C), exhibiting great potential for actuator and sensor applications.