The exciting combination of high electrical conductivity, high specific capacitance and colloidal stability of two-dimensional Ti3C2Tx MXene (referred to as MXene) has shown great potential in a wide range of applications including wearable electronics, energy storage, sensors, and electromagnetic interference shielding. To realize its full potential, recent literature has reported a variety of solution-based processing methodologies to develop MXenes into multifunctional architectures, such as fibres, films and aerogels. In response to these recent critical advances, this review provides a comprehensive analysis of the diverse solution-based processing methodologies currently being used for MXene-architecture fabrication. A critical evaluation of the processing challenges directly affecting macroscale material properties and ultimately, the performance of the resulting prototype devices is also provided. Opportunities arising from the observed and foreseen challenges regarding their use are discussed to provide avenues for new designs and realise practical use in high performance applications.