The pursuit of geometrically frustrated lattices beyond conventional paradigms remains a central challenge in the design of quantum materials. Herein, we report the discovery of the A3V9Te13 (A = Cs, Rb) family of vanadium-based intermetallic compounds, which host a unique two-dimensional Mosaic lattice derived from the Kagome network, composed of an ordered tessellation of triangles, squares, and pentagons. The Cs compound (CVT) exhibits strong electronic correlations, characterized by non-Fermi liquid behavior at low temperatures, an exceptionally large Sommerfeld coefficient, and a bulk phase transition at T* ≈ 47 K with possible charge- or spin-related origin. Inspired by pressure-tuning in related Kagome systems, we demonstrate that the electronic ground state of this lattice is exquisitely tunable via chemical pressure. Systematic substitution of Cs with smaller Rb ions suppresses the T* phase transition and the correlated electronic response, ultimately driving the system into a highly frustrated semiconducting ground state without long-range magnetic order down to 60 mK. This work unveils a new structural platform for exploring the interplay between geometric frustration and strong electron correlations, providing a chemically controllable platform for exploring the phase space between distinct correlated electronic states.