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In this work, the coexistence of In(III) and K(I) induces a rapid crystal growth of single crystals of heterometallic metal-organic frameworks (MOFs), [In0.5K(3-qlc)Cl-1.5(H2O)(0.5)](2n) (1) and [InK(ox)(2)-(H2O)(4)](n) (2) (3-Hqlc = quinoline-3-carboxylic acid; H(2)ox = oxalic acid). Remarkably, with the help of achiral 3-Hqlc, compound 1 represents the chiral interpenetrating p-block heterometallic MOFs with helical chain along the 43 screw axis, while compound 2 possesses a highly symmetric (4,4,4)-connected topology network with a Schlafli symbol of (4(2).8(3).10))(4(2).8(4)). Consideration of two different organic ligands viz. 3-Hqlc and H(2)ox constructed heterometallic MOFs with different geometrical dimensions of unit cells, their influences on luminescence arid photovoltaic properties are studied. Compounds 1 and 2 show tunable luminescence from blue to yellow and white by varying the temperature in the solid state. Encouraged by the UV visible absorption and HOMO-LUMO energy states matched for sensitizing TiO2, the two compounds are employed in combination with N719 in dye-sensitized solar cells (DSSCs) to compensate for absorption in the region of ultraviolet and blue-violet. Under optimized conditions, the DSSCs devices using cosensitizers of 1/N719 and 2/N719 display an overall conversion efficiency of 8.07% and 7.42%, which is 22.09% and 12.25% higher than that of a device solely sensitized by N719 (6.61%). Consequently, both of the two compounds could serve as excellent photosensitizers and application in luminescence sensors and DSSCs.