This study is a pilot exploration to develop rigorous, green, intellectualized approach for optimal controlling the 3D concrete printing. The mechanical performances of 3D printed samples during super-early age, early age, and hardened state are tested and monitored using piezoelectric zirconate titanate (PZT) patches. EMI sensing technique is applied to quantify stiffness gain of printed concrete to evaluate the structural build-up behaviour by establishing the instant correlation between the stiffness of concrete and the EMI signatures. An optimization method for printing process based on EMI detection is proposed. In this way, the PZT signals can be feedback to the digital control system of printer in real time to adjust the printing setting. Instant intellectualization for the 3D printing technique is then realized and the buildability of the printed concrete is expected to be improved. The different early age properties of both printed and casted composites are elaborated. Thereafter, changes of frequency and amplitude in the conductance spectrum acquired by mounted PZT patches are employed to characterize and quantify the mechanical behaviours of the 3D printed samples exposed to orthogonal loadings, which contribute to the understanding of damage accumulation and failure process of concrete materials.