Three-dimensional (3D) ferroelectric materials are promising electromechanical building blocks for achieving human-machine interfacing, energy sustainability, and enhanced therapeutics. However, current natural or synthetic materials cannot offer both high piezoelectric responses and desired mechanical toughness at the same time to meet the practicality. Here, a nacre-mimetic ferroelectric metamaterial was created with a ceramic-like piezoelectric property and a bone-like fracture toughness through electric-field-assisted 3D printing. The as-printed bulk structure, consisting of periodically intercalated soft ferroelectric and hard electrode layers, exhibited a giant d33 of over 130 pC/N, as well as a superior fracture resistance of ~ 5.5 MPa·m1/2, more than three times higher than conventional piezo-ceramics. The excellent printability together with the unique combination of both high piezoelectric and mechanical behaviors allowed us to create artificial piezoelectric bones with tunable anisotropic piezoelectricity and bone-comparable mechanical properties, marking a cornerstone toward manufacturing practical, high-performance, and smart biological systems.