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This paper presents a study and comparison of surface effects induced by picosecond and nanosecond laser modification of a Ti6Al4V alloy surface under different ambient conditions: air and argon- and nitrogen-rich atmospheres. Detailed surface characterization was performed for all experimental conditions. Damage threshold fluences for picosecond and nanosecond laser irradiation in all three ambient conditions were determined. The observed surface features were a resolidified pool of molten material, craters, hydrodynamic effects and parallel periodic surface structures. Laser-induced periodic surface structures are formed by multi-mode-beam nanosecond laser action and picosecond laser action. Crown-like structures at crater rims are specific features for picosecond Nd:YAG laser action in argon-rich ambient conditions. Elemental analysis of the surfaces indicated nitride compound formation only in the nitrogen-rich ambient conditions. The constituents of the formed plasma were also investigated. Exploring the impact of process control parameters on output responses has been undertaken within the context of laser modification under different environmental conditions. Parametric optimization of the nanosecond laser modification was carried out by implementing an advanced method based on Taguchi’s parametric design and multivariate statistical techniques, and optimal settings are proposed for each atmosphere.