Ti6Al4V (Ti64) is a versatile material, finding applications in a wide range of industries due to its unique properties. However, hydrogen embrittlement (HE) poses a challenge in hydrogen-rich environments, leading to a notable reduction in strength and ductility. This study investigates the complex interplay of solute hydrogen (SH) and hydride phase (HP) formation in Ti64 by employing two different current densities during the charging process. Nanoindentation measurements reveal distinct micro-mechanical behavior in base metal, SH, and HP, providing crucial insights into HE mechanisms affecting macro-mechanical behavior. The fractography and microstructural analysis elucidate the role of SH and HP in hydrogen-assisted cracking behaviors. The presence of SH heightens intergranular cracking tendencies. In contrast, the increased volume of HP provides sites for crack initiation and propagation, resulting in a two-layer brittle fracture pattern. The current study contributes to a comprehensive understanding of HE in Ti6Al4V, essential for developing hydrogen-resistant materials.