By analyzing (2712.4±14.3)×106 ψ(3686) events collected with the BESIII detector operating at the BEPCII collider, we report the first observation of χcJ→ΛKS0Ξˉ0+c.c. (J=0,1,2) with significances greater than 10σ, including systematic uncertainties, and improved measurements of χcJ→ΛK−Ξˉ++c.c. The branching fractions of these decays are determined to be B(χc0→ΛKS0Ξˉ0+c.c.)=(1.13±0.13±0.13)×10−4, B(χc1→ΛKS0Ξˉ0+c.c.)=(0.74±0.08±0.07)×10−4, B(χc2→ΛKS0Ξˉ0+c.c.)=(1.16±0.11±0.14)×10−4, B(χc0→ΛK−Ξˉ++c.c.)=(1.90±0.08±0.16)×10−4, B(χc1→ΛK−Ξˉ++c.c.)=(1.40±0.05±0.11)×10−4, and B(χc2→ΛK−Ξˉ++c.c.)=(1.95±0.07±0.15)×10−4. The first uncertainties are statistical, and the second are systematic.