The ASA process enables the recycling, repairing, and reprogramming of high-performance organic aerogels. This method involves breaking down polyimine aerogels into a solution of oligomers through transamination reactions with amines, followed by reassembly into new aerogels. The process is highly selective, reproducible, and resource-efficient, conserving 100% of the original chemical resources. It allows for the creation of new aerogels with identical properties to the original ones, even from mixed waste streams or damaged materials. The process also enables post-synthetic reprogramming of aerogel properties by introducing different amines, leading to enhanced hydrophobicity, thermal conductivity, and mechanical performance. The ASA process is applicable to various aerogel types and can be used to repair aerogels damaged by chemicals or force. The resulting aerogels maintain their structural integrity and performance, demonstrating the potential for sustainable management of thermally insulating materials. The study highlights the versatility of the ASA process in creating sustainable, high-performance aerogels with applications in energy-efficient insulation.The ASA process enables the recycling, repairing, and reprogramming of high-performance organic aerogels. This method involves breaking down polyimine aerogels into a solution of oligomers through transamination reactions with amines, followed by reassembly into new aerogels. The process is highly selective, reproducible, and resource-efficient, conserving 100% of the original chemical resources. It allows for the creation of new aerogels with identical properties to the original ones, even from mixed waste streams or damaged materials. The process also enables post-synthetic reprogramming of aerogel properties by introducing different amines, leading to enhanced hydrophobicity, thermal conductivity, and mechanical performance. The ASA process is applicable to various aerogel types and can be used to repair aerogels damaged by chemicals or force. The resulting aerogels maintain their structural integrity and performance, demonstrating the potential for sustainable management of thermally insulating materials. The study highlights the versatility of the ASA process in creating sustainable, high-performance aerogels with applications in energy-efficient insulation.