Comparison of three-dimensional (3D) printing and cast methods on the mechanical properties of cementitious materials is the basis for intelligent construction development. To achieve this, a series of experiments including the uniaxial tensile, compressive, flexural and interlayer bonding tests of mould-cast and 3D printed (3DP) specimens are conducted to investigate the effects of different preparation technologies on the microstructure and hardening properties of limestone calcined clay cement (LC3) based engineered cementitious composites (ECC). Results indicate that the tensile strength and strain capacity of the printed LC3-ECC decrease by 16.6%–22.7 % and 43.3%–54.6 % compared to the cast specimens, while it still possesses a strain capacity of 2 % and multiple cracking behaviour. The compressive and flexural properties of the printed LC3-ECC both show significant anisotropy, the maximum values of which are observed in the Z- and Y- directions, respectively. The interlayer bonding strength increases by 54.3%–91.9 % at 28 d compared to that at 7 d due to the hydration of LC3. The pore structure of the printed LC3-ECC is denser than that of the cast LC3-ECC, with more regular arrangement and finer size of pores. The macro-micro properties correlation analysis proves the better comprehensive performance of printed LC3-ECC relative to casted LC3-ECC, as well as reveals the relationship between pore structure and anisotropy. In terms of material sustainability, 3DP-LC3-ECC has a significant reduction in energy and carbon emissions compared to typical M45-ECC, contributing to the environmental development.