In modern materials research, nanotechnology will play a game-changing role, with nanoarchitectonics as an overarching integrator of the field and artificial intelligence hastening its progress as a super-accelerator. We would like to discuss how this schema can be utilized in the context of specific applications, with exemplification using disease diagnosis. In this paper, we focus on early, noninvasive disease diagnosis as a target application. In particular, recent trends in chemosensing in the detection of cancer and Parkinson’s disease are reviewed. The concept has been gaining traction as dynamic volatile metabolite profiles have been increasingly associated with disease onset, making them promising diagnostic tools in early stages of disease. We also discuss advances in nanoarchitectonic chemosensors, which are theoretically ideal form factors for diagnostic chemosensing devices. Last but not least, we shine the spotlight on the rise to prominence and emergent contributions of artificial intelligence (AI) in recent works, which have elucidated a strong synergy between chemosensing and AI. The powerful combination of nanoarchitectonic chemosensors and AI could challenge our current notions of disease diagnosis. Disease diagnosis and detection of emerging viruses are important challenges facing society. The parallel development of advanced functional materials for sensing is necessary to support and enable AI methodologies in making technological leaps in applications. The material and structural formative technologies of nanoarchitectonics are critical in meeting these challenges.