Aerogels are materials with high porosity, high surface area, very low density, and low conductivity. General inorganic aerogels such as silica aerogels have been widely studied for their excellent thermal insulation properties, but their use is limited due to poor mechanical properties. To overcome these difficulties, organic aerogels such as polyimide aerogels having excellent mechanical properties and high temperature safety are drawing attention. Polyimide (PI) has been applied as an engineering material due to its high thermal stability, excellent mechanical properties, and outstanding chemical resistance. Despite of these excellent properties, research to improve their physical properties and thermal properties is still ongoing. For the purpose, in our work, we prepared PI composite aerogels by adding materials such as carbon nanotubes (CNTs) and 1,3,5-Tris(4-aminophenoxy) benzene (TAB). CNTs offer the potential to confer electrical properties upon the manufactured PI composite aerogels. TAB serves as an effective crosslinking agent, imparting low shrinkage, high porosity, improved mechanical strength, and enhanced thermal characteristics to the aerogels. In this work, PI aerogels were successfully manufactured using a cost-effective and eco-friendly approach that included freeze-drying and thermal imidization. The electrical and mechanical properties vary depending on the materials added, and the changes were observed by focusing on the gauge factor (GF) and sensitivity (S), which are indicators to evaluate the performance of the sensor. The fabricated PI composite aerogel has shown promising improvements suitable for pressure sensors that can adapt to various environmental conditions. Structural and mechanical analyses of the PI composite aerogels were conducted utilizing scanning electron microscopy (SEM), universal testing machine (UTM), and thermogravimetric analysis (TGA). Electrical analyses were performed using a multimeter. The comprehensive assessment revealed that the PI composite aerogels exhibit superior mechanical and thermal properties compared to additive-free PI aerogels. This suggests their potential utility as lightweight, high-performance materials, with wide sensing ranges and high sensitivity, particularly advantageous for their application as pressure sensors.