Synthetic dyes, such as methylene blue (MB) and methyl orange (MO), are widely released from textile industries and pose a serious global health concern due to their carcinogenic and mutagenic properties, threatening public health and disrupting natural ecosystems. In this study, titanium-nickel nanocomposites (Ti-Ni NCs) were synthesized using the pulse laser ablation in liquid (PLAL) method for efficient dye removal applications. The optical and chemical properties of TiO₂ NPs, NiO NPs, and Ti-Ni NCs were characterized using ultraviolet-visible (UV-Vis), fluorescence (FL), and Fourier-transform infrared (FTIR) spectroscopy. The UV-Vis spectra exhibited a prominent absorption peak at ~361 nm in the UV region, while Tauc plot analysis showed a significant bandgap blue shift upon incorporation of NiO into TiO₂ NPs. FTIR spectra showed the presence of Ti-O, Ni-O, and Ti-O-Ni vibrational bands, proving the interfacial interaction between TiO₂ and NiO upon mixing. The Ti-Ni NCs revealed enhanced photocatalytic activity, achieving up to 97.1% degradation of MB and 89.6% MO removal within 45 minutes, showing advanced photocatalytic properties under UV light irradiation. This enhancement is attributed to the synergistic effect between TiO₂ and NiO, which forms a p-n heterojunction, effectively improving charge separation efficiency. These findings proposed the potential of high-purity PLAL-synthesized Ti-Ni NCs as advanced photocatalysts for wastewater remediation.