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Skyrmions with multiple helicity or topology in centrosymmetric crystals are intriguing magnetic-domain objects due to their diverse dynamics under external stimuli. Here we illustrate how the two key gradients of magnetocrystalline anisotropy (MCA) and spin reorientation transition (SRT) affect the skyrmion formation and topology by Cu substitution in the biskyrmion-host MnNiGa alloy. The MCA and SRT are simultaneously tuned in a large scope, while the original high Curie temperature (${T}_{C}$) is retained. Detailed neutron-scattering studies revealed the construction of a noncollinear canted magnetic structure below the SRT temperature (${T}_{\mathrm{SR}}$), which effectively correlates the SRT with the evolution of the MCA, as well as the exchange interaction. The Cu substitution raises the ${T}_{\mathrm{SR}}$ to merge with the ${T}_{\mathrm{C}}$, and meanwhile, reduces the $c$-axis anisotropy. Lorentz transmission electron microscopy revealed the formation of stacked biskyrmions from above room temperature to lower temperatures in $\mathrm{MnN}{\mathrm{i}}_{1\ensuremath{-}x}\mathrm{C}{\mathrm{u}}_{x}\mathrm{Ga}\phantom{\rule{0.28em}{0ex}}(x=0--0.3)$ in the presence of proper MCA. Micromagnetic simulations further confirmed the great effect of uniaxial anisotropy on the stabilization of biskyrmions. Our work has helped clarify the evolution of magnetic structures and their correlation to the SRT, providing an account of the effect of MCA and exchange interaction on the biskyrmion formation.

physical review. b./physical review. b

Simultaneous tuning of magnetocrystalline anisotropy and spin reorientation transition via Cu substitution in Mn-Ni-Ga magnets for nanoscale biskyrmion formation