Hydrogen embrittlement of Ti6Al4V alloy was investigated under electrochemical cathodic hydrogen charging. Advanced surface treatment and material characterisation, laser shock peening (LSP) or laser peening (LP), atom probe tomography, slow strain rate tensile (SSRT) test, and XRD residual stress are employed for analysis. Results obtained exposed the opportunity to implement surface treatment for controlling hydrogen embrittlement. Induced grain refinement and compressive residual stress restrict the hydrogen uptake in Ti6Al4Valloy. Furthermore, APT results gave wt. % of TiH (titanium hydride) in laser peened hydrogen charged and untreated hydrogen-charged specimens. Thus, it is concluded that compressive stress induced by laser peening process controlled uptake of hydrogen by Ti6Al4V alloy. © 2021, The Author(s), under exclusive licence to Springer-Verlag London Ltd., part of Springer Nature.