We propose using a slide-ring (SR) gel electrolyte to achieve a gel polymer electrolyte with both sufficient mechanical strength and high ionic conductivity. The SR gel is made from polyrotaxane, which has a structure that consists of cyclic molecules, α-cyclodextrins (CDs), threaded by an axial polymer chain, polyethylene glycol (PEG), and cross-linked by divinyl sulfone. The SR gel electrolyte was made from SR gels which were swollen by an electrolyte solution (ES) prepared with lithium salt and 1-ethyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide (EMITFSI). The swelling behavior of SR gel in the ES by the formation of coordination bonds between lithium cations and oxygen atoms on CDs was investigated. The swelling behavior and ionic conductivity of the SR gel swollen with ES had a peak at 0.8M lithium ion in the ES and the molar conductivity of the SR gel swollen with ES was 85% more than that of pristine ES. The puncture resistance of the SR gel electrolyte was also investigated; the puncture elongation was more than 1000% and the Young’s modulus increased with the lithium ion concentration due to an increase in the coordination bonds between lithium cations and the oxygen atoms on CDs.