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The increasing demand for miniaturized, wearable, and flexible electronics has promoted the development of micro power sources such as microsupercapacitors (MSCs). This work reports a high-performance MSC based on Ti3C2Tx-layer/MnO2-nanorod with an ionic liquid gel electrolyte, achieving a high areal capacitance of 24.7 mF cm−2 within a wide voltage window of 2.5 V. The specific layer–rod interlaced structure of Ti3C2Tx/MnO2 is designed to solve the inaccessibility of large-sized ions in ionic liquids into Ti3C2Tx layers. As a result, the structure modification provides an enhanced capacitance because the expanded interspace enables a sufficient number of large-sized ions to intercalate/deintercalate. This work provides insightful guidance for the interlaminar modification of Ti3C2Tx MXene to accommodate high operating voltage electrolyte with large-sized ions to obtain high-performance MSCs.