Boc(Boc= tert-butoxycarbonyl)-p-nitro-L-phenylalanyl-p-nitro-L-phenylalanine, a dipeptide characterized by acentric symmetry, self-assembles into micro-tapes. This study explores its thermal, structural, and nonlinear optical properties. Thermo-gravimetric analysis reveals an onset degradation temperature of 190 ºC, with primary and secondary peaks at 202 ºC and 220 ºC, respectively. The crystal structure of the dipeptide was determined through single crystal X-ray diffraction at 100 K, confirming its crystallization in space group P2 with two molecules per unit cell. Additionally, optical second harmonic generation polarimetry indicates a significant nonlinear optical response, with an effective coefficient (deff) estimated to be at least 0.52 pm/V. This value is only four times lower than that of state-of-the-art phase-matched β-barium borate nonlinear crystals, highlighting the potential of this dipeptide in nonlinear optical applications.