Hydrogen’s effect on the shape memory effect (SME) of [1¯17]-oriented Ti49.7-Ni50.3 (at.%) alloy single crystals, with a B2–B19′ martensitic transformation (MT), was studied after being electrolytically hydrogenated at a current density of 1500 A/m2 for 3 h at room temperature under isobaric tensile deformation. It was shown that, under the used hydrogenation regime, hydrogen was in a solid solution and lowered the elastic modulus of B19′ martensite. The hydrogen in a solid solution increased (i) the yield strength σ0.1 of the initial B2 phase by 100 MPa at Md temperature, (ii) the σ0.1 of the stress-induced B2–B19′ MT by 25 MPa at Ms temperature, and (iii) the plasticity of B19′ martensite relative to the hydrogen-free crystals. At the same level of external stresses, the SME in the hydrogenated crystals was greater than that in hydrogen-free crystals. At external tensile stresses σex = 200 MPa, the SME was 4.4 ± 0.2% in the hydrogenated crystals and 1.8 ± 0.2% without hydrogen. Hydrogen initiated a two-way SME of 0.5 ± 0.2% at σex = 0 MPa, which was absent in the hydrogen-free crystals. The physical reasons leading to an increase in the SME upon hydrogenation are discussed.