Nickel catalysts have recently played an important role for rapidly and reliably converting feedstock chemicals into valuable compounds of interest for both pharmaceutical and academic laboratories. Herein, we summarize the recent advances on the ability of nickel catalysts to trigger olefin isomerization via “chain‐walking”, causing a displacement of the nickel catalyst throughout the alkyl chain while opening up new grounds for forging C−C and C‐heteroatom linkages at remote, yet unfunctionalized, sp³ C−H bonds.