Self-powered photodetection driven by ferroelectric polarization has shown great potential in next-generation optoelectronic devices.H ybrid perovskite ferroelectrics that combine polarization and semiconducting properties have ap romising position within this portfolio.H erein, we demonstrate the realization of self-powered photodetection in an ew developed biaxial ferroelectric,( EA) 2 (MA) 2 Pb 3 Br 10 (1,E Ai s ethylammonium and MA is methylammonium), whichd isplaysh igh Curie temperature (375 K), superior spontaneous polarization (3.7 mCcm À2 ), and unique semiconducting nature. Strikingly,w ithout an external energy supply, 1 exhibits an direction-selectable photocurrent with fascinating attributes including high photocurrent density ( % 4.1 mAcm À2 ), high on/ off switching ratio (over 10 6 ), and ultrafast response time (96/ 123 ms);s uch merits are superior to those of the most active ferroelectric oxide BiFeO 3 .F urther studies reveal that strong inversion symmetry breaking in 1 provides adesirable driving force for carrier separation, accounting for such electrically tunable self-powered photoactive behaviors.T his work sheds light on exploring new multifunctional hybrid perovskites and advancing the design of intelligent photoelectric devices.Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.