A portable sensor with an optical case dimension of 46 × 28 × 16 cm3 based on laser absorption spectroscopy for highly sensitive measurement of formaldehyde was reported. A compact improved spherical mirror multi-pass cell consisting of two 5-cm diameter spherical mirrors separated by 17.7 cm was developed. The cell offered a sample volume of 350 mL and an optical absorption path length of 50.6 m, giving a high path length-to-volume ratio of 14.6 cm−2. The sampling response time was less than 1 s, allowing the application of rapid spectral background subtraction technique to effectively suppress optical fringes. The achieved detection limit was 650 pptv (1σ, 1 s), corresponding to a minimum detection absorption coefficient of 2.3 × 10−9 cm−1. The capability of the HCHO sensor was demonstrated by two days of continuous indoor air monitoring. The developed portable sensor is suitable for mobile and fast indoor air quality measurements.