Pintle injectors offer variable thrust capability and combustion stability advantages for liquid rocket engines. This study presents experimental and numerical investigation of spray characteristics for a liquid–liquid pintle injector using water as simulant. Ten cold flow tests covering total momentum ratio (TMR) from 0.36 to 2.76 captured spray angle variations from 26° to 80°. Computational fluid dynamics (CFD) simulations using Ansys Fluent 2025 R1 with the Volume of Fluid method and dispersed interface modeling showed good agreement with experimental spray angles for TMR > 0.74 (error < 8%), but demonstrated increasing discrepancy at lower TMR values (up to 62% error at TMR = 0.36). This deviation indicates limitations of steady-state RANS models in capturing unsteady, fuel-dominated flow regimes. The experimental dataset provides validation benchmarks for CFD modeling and contributes to injector design optimization for sounding rocket applications.