Here, weaddress this challenge through a combination of protein engineering,native ion mobility mass spectrometry, and molecular dynamics simulations.We used an LLPS-compatible spider silk domain and pH changes to controlthe self-assembly of the hnRNPs FUS, TDP-43, and hCPEB3, which areimplicated in neurodegeneration, cancer, and memory storage. The gene discussed is TARDBP; the disease is cancer.