The recent technological and methodological developments in NMR spectroscopy have dramatically decreased its detection limit, hence expanding its application areas. Herein, we report the first experimental detection of (2)H-(13)C isotopomeric isomers (isotopomers) in natural abundance (1.7 × 10(-4)%) both in liquids and oriented systems by combining cryoprobe, high magnetic field, and carefully chosen 2D heteronuclear correlation techniques. These experimental results require the detection of one molecule among 600,000 and demonstrate the sensivity and the selectivity of the employed NMR techniques. Besides, we show that (2)H-(13)C enantio-isotopomers can be distinguished using 2D NMR in chiral polypeptide alignment media, thus providing a new tool for the chiral analysis. This method opens fruitful propects in various analytical fields such as molecular source authentication, metabolism studies, or the fight against counterfeiting.