Amorphous titanium tetrasulfide (TiS₄) is investigated as a high-capacity cathode material for sulfide-based solid-state batteries using Li₆PS₅Cl argyrodite as solid electrolyte. A systematic comparison between low-energy ball milling (LBM) and high-energy ball milling (HBM) reveals that tribochemical processing intensity determines composite microstructure and electrochemical performance. HBM-processed composites exhibit superior homogenization confirmed by quantitative FIB-SEM analysis, achieving discharge capacities of 1110 mAh g_S⁻¹ at 0.05 C and 669 mAh g_S⁻¹ at 0.5 C. Despite lower bulk electronic conductivity, HBM composites demonstrate enhanced performance consistent with shortened solid-state diffusion lengths and increased triple-phase boundary density. SOC-dependent electrochemical impedance spectroscopy reveals that HBM composites accumulate only 19% impedance growth at 100% SOC over 34 cycles compared to 41% for LBM counterparts, indicating superior interfacial stability. Time-of-flight secondary ion mass spectrometry provides spatial evidence for heterogeneous lithiation, with codetected TiS⁺ and Li₃S⁺ species consistent with gradual structural reorganization along the conversion trajectory. Scalability is demonstrated through dry-film electrode fabrication, and HBM-processed cathodes achieve initial capacities of 1240 mAh g_S⁻¹ and retain 950 mAh g_S⁻¹ after 80 cycles. Absolute capacity values reflect the combined electrochemistry of TiS₄ and partially decomposed Li₆PS₅Cl. This work establishes tribochemical processing as a viable strategy for optimizing conversion-type cathodes in solid-state batteries.