AbstractImproving the accessibility of ions in the electrodes of electrochemical energy storage devices is vital for charge storage and rate performance. In particular, the kinetics of ion transport in organic electrolytes is slow, especially at low operating temperatures. Herein, we report a new type of MXene-carbon nanotube (CNT) composite electrode that maximizes ion accessibility resulting in exceptional rate performance at low temperatures. The improved ion transport at low temperatures is made possible by breaking the conventional horizontal alignment of the two-dimensional layers of the MXene Ti₃C₂ by using specially designed knotted CNTs. The large, knot-like structures in the knotted CNTs prevent the usual restacking of the Ti₃C₂ flakes and create fast ion transport pathways. The MXene-knotted CNT composite electrodes achieve high capacitance (up to 130 F g⁻¹ (276 F cm⁻³)) in organic electrolytes with high capacitance retention over a wide scan rate range of 10 mV s⁻¹ to 10 V s⁻¹. This study is also the first report utilizing MXene-based supercapacitors at low temperatures (down to −60 °C).