Acyl thioureas are versatile organosulfur scaffolds with broad relevance in coordination chemistry and functional applications, driven by their structural flexibility and the presence of both hard and soft donor sites. This enables the formation of diverse metal complexes with tunable properties. This review provides a critical overview of recent advances (2024–2026) in their synthesis, conformational features, coordination behavior, and applications. Emphasis is placed on structure–activity and coordination–property relationships, highlighting how substituent effects and coordination modes influence biological, catalytic, and agrochemical performance. In addition, coordination behavior is systematically classified to improve understanding of structure–function correlations. The current review integrates recent experimental and computational findings to identify key trends and challenges, offering insights for the rational design of acyl thiourea-based systems for advanced applications.