ABSTRACT Ferroelectric materials exhibit great potential for nonlinear optical applications due to their robust second‐order nonlinear optical responses. Strain engineering of such materials has demonstrated significant enhancement of second‐harmonic generation (SHG) responses. However, achieving order‐of‐magnitude amplification in bulk crystals and understanding anisotropic strain‐property relationships remain challenging. Here, we report strong SHG enhancement in anisotropically strained ferro