The use of cementitious piezoelectric composite enables structure monitoring of concrete construction, while its piezoelectric and mechanical performance are relatively low. This paper developed a novel high-performance piezoelectric composite through carbonation of calcium and magnesium-based binder (including Ca(OH)2 and Mg(OH)2). The influence of PZT volume, forming regime, and polarization condition on compressive strength and piezoelectric strain coefficient (d33) of the two piezoelectric composites was investigated. Results showed that the use of PZT volume from 20 % to 80 % led to a 6-fold and 3-fold greater d33 value for Ca(OH)2 and Mg(OH)2 piezoelectric composites, respectively. While, such change in PZT volume reduced the compressive strength by 50 % and 55 % for the two piezoelectric composites. This is due to the significantly increased porosity and decreased carbonation degree as indicated by microstructural analysis. The use of a higher forming pressure from 25 to 100 MPa resulted in 60 % and 105 % increases in d33 values for the two piezoelectric composites. Such improvements in compressive strength were 120 % and 135 %, respectively. The d33 values were increased by 45 % and 60 % with the polarization voltage increasing from 1.5 to 3.5 kV/mm for the two piezoelectric composites. Such increases in d33 were 64 % and 94 % when polarization duration extended from 5 to 25 min. This study determined the optimal preparation regime of the two piezoelectric composites that can ensure the best overall performance considering the trade-off among piezoelectric, mechanical, and microstructural properties of the composites. The results of this paper can facilitate the application of novel and high-performance of piezoelectric sensor in smart concrete structures.