Aerogels with air-filled pores and interconnected 3D solid networks show unique characteristics and, therefore, have tremendous applications in various fields. Integrating specific characteristics of aerogels, large surface area, low density, and high porosity are included which opens up possibilities for new application areas. Aerogels' advanced features provide high selectivity and sensitivity, fast recovery and response to sensing materials in sensors such as biosensors, gas, pressure, and strain sensors. In recent years significant work has been done regarding the development of aerogel-based sensors. In this chapter, recent challenges and some approaches to high-performance aerogel-based sensor development are summarized.