Herein, we present a novel cage-cluster-based framework composed of Ti₄L₆ (L = embonate) tetrahedra and [Pb₄(µ₃-OH)₄]⁴⁺ cubane-like clusters that also exhibits high stability in water, air, and other common solvents. According to the topology study, it exhibits a chiral srs-type network. Integrating titanium cages and lead-oxo clusters into a rigid cage-cluster-based framework significantly enhances its third-order nonlinear optical (NLO) property.