MXene　aerogels,　known　for　good　electrical　properties,　offer　immense　potential　for　the　development　of　high-sensitivity　pressure　sensors.　However,　the　intrinsic　challenges　stemming　from　the　poor　self-assembly　capability　and　high　hydrophilicity　of　MXene　impede　the　natural　drying　process　of　MXene-based　hydrogels,　thereby　constraining　their　application　on　a　large　scale　in　sensor　technology.　Herein,　a　graphene-assisted　approach　aimed　at　modulating　the　hydrophobicity　and　enhancing　framework　strength　of　MXene　through　a　well-designed　prefreezing　technique　incorporating　3D　spherical　macroporous　structures　is　proposed.　This　synergistic　strategy　enables　the　fabrication　of　naturally　dried　MXene　aerogels　across　various　size　scales.　Moreover,　the　integration　of　3D　spherical　macroporous　structures　improves　elasticity　and　electrical　responsiveness　of　aerogels.　Consequently,　the　aerogel　sensor　exhibits　great　performances,　including　high　sensitivity　(1250　kPa−1),　low　detection　limit　(0.4 Pa),　wide　frequency　response　range　(0.1–8 Hz),　and　excellent　stability　(1000　cycles).　This　sensor　proves　adept　at　monitoring　pressure　signals　ranging　from　lightweight　paper　to　human　motion.　Additionally,　the　application　of　customized　laser　engraving　endows　aerogels　with　unique　functionalities,　such　as　compressibility　and　immunity　to　strain,　stretchability　and　resistance　to　compression,　as　well　as　wind　detection.　Thus,　the　proposed　approach　holds　significant　promise　as　a　scalable　method　for　the　mass　production　of　aerogels　with　versatile　applications.　©　2024　Wiley-VCH　GmbH.