emission, noiseless, friendliness for miniaturization, and reliability. [1,2] Based on the Seebeck and Peltier effects, thermoelectricity enables a direct energy conversion between temperature difference and electricity. [3] The performance of a TE material is primarily gauged by the material's figure of merit, zT = α 2 T/ρκ, where α is the Seebeck coefficient, T is the absolute temperature, ρ is the electrical resistivity, and κ is the total thermal conductivity (consisting of the lattice thermal conductivity κ L and the electronic thermal conductivity κ E ).In view of the adversely interdependent S, ρ, and κ, attaining high zT values entails hierarchical diverse structurefunctional modules in the material. To this end, "hybrid crystal" or "structural modularity" is preferred in TE materials research as these complex materials are composed of building modules with distinct compositions and functions, [4,5] through which the adverse coupling of S, ρ, and κ can be eased and tuned selectively. Layered cobalt oxides, [6] filled skutterudites, [7] meta-phases, [8] and liquid-like TE materials [9] are good examples To date, thermoelectric materials research stays focused on optimizing the material's band edge details and disfavors low mobility. Here, the paradigm is shifted from the band edge to the mobility edge, exploring high thermoelectricity near the border of band conduction and hopping. Through coalloying iodine and sulfur, the plain crystal structure is modularized of liquid-like thermoelectric material Cu 2 Te with mosaic nanograins and the highly size mismatched S/Te sublattice that chemically quenches the Cu sublattice and drives the electronic states from itinerant to localized. A state-of-the-art figure of merit of 1.4 is obtained at 850 K for Cu 2 (S 0.4 I 0.1 Te 0.5 ); and remarkably, it is achieved near the Mott-Ioffe-Regel limit unlike mainstream thermoelectric materials that are band conductors. Broadly, pairing structural modularization with the high performance near the Mott-Ioffe-Regel limit paves an important new path towards the rational design of high-performance thermoelectric materials.