By developing the sensitivity of our custom‐made spectrometer, we have succeeded for the first time in detecting the strains in an Al0.3Ga0.7As/GaAs heterostructrued sample through Al nuclear spins based on standard nuclear magnetic resonance (NMR) technique. By analyzing the observed quadrupolar‐split frequency value, it is concluded that the strain is dominantly caused by the lattice mismatch around the interface, rather than the contraction of epoxy resin that bundles the sample. (© 2011 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)