Nonlinear-optical (NLO) crystals capable of controlling and manipulating light to generate coherent radiation at challenging wavelengths are of significant interest. However, designing a new UV NLO crystal remains difficult due to the rigid requirements for structure and properties. Herein, we have successfully designed and synthesized a novel noncentrosymmetric (NCS) rare-earth borate UV NLO crystal, K3Y3(BO3)4, through the heterovalence substitution of YAl3(BO3)4. K3Y3(BO3)4 (KYBO) crystallizes in the NCS and polar space group of P63mc, with the structure formed by the interconnectioned BO3 triangles and YO8 polyhedra through corner-sharing and edge-sharing. The property measurements indicate that KYBO is second-harmonic-generation-active with a moderate response, ∼2 × KDP. Meanwhile, KYBO can exhibit a short UV cutoff edge (λcutoff < 190 nm), indicating its potential as a new UV or deep-UV NLO crystal.