Aim: Early detection and removal of colorectal cancer (CRC) and advanced adenomas (AAs) decreases the incidence of and mortality from the disease. We aimed to evaluate the potential of faecal volatile organic compounds (VOCs) for detection and follow-up of colorectal adenoma using advanced electronic nose technology. Method: This was a prospective multi-centre case–control cohort including two district hospitals and one tertiary referral hospital. Patients undergoing colonoscopy were instructed to collect a faecal sample prior to bowel cleansing and were included in the study when CRC, AAs, large adenomas (LAs; 0.5–1.0 cm), small adenomas (SAs; 0.1–0.5 cm) or no endoscopic abnormalities (controls) were observed. Patients undergoing polypectomy and controls were asked for a second sample after 3 months. Faecal VOCs were measured with gas chromatography–ion mobility spectrometry. Random forest, support vector machine, Gaussian process and neural net classification were used to evaluate accuracy. Results: In total, 14 patients with CRC, 64 with AAs, 69 with LAs, 127 with SAs and 227 controls were included. A second sample was collected from 32 polypectomy patients and 32 controls. Faecal VOCs discriminated CRC and adenomas from control [AUC (95% CI): CRC vs control 0.96 (0.89–1); AA vs control 0.96 (0.93–1); LA vs control 0.96 (0.92–0.99); SA vs control 0.96 (0.94–0.99)]. There were no significant differences between CRC and adenoma groups. Patients with adenomas and controls were discriminated prior to polypectomy, whereas 3 months after polypectomy VOC profiles were similar [T0 adenoma vs control 0.98 (0.95–1); T1 adenoma vs control 0.55 (0.40–0.69)]. Conclusions: Faecal VOC profiles may be useful for early detection of CRC and adenomas and the timing of polyp surveillance as polypectomy led to a normalization of the VOC profile.