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The feasibility of ultrafast high‐resolution intermolecular multiple‐quantum coherence (UF‐iMQC) spectroscopy for the direct analysis of molecular‐mobility‐restricted samples that are not suitable for magic‐angle spinning, such as a jelly, hand soap, and marrow, is presented. Most components could be directly detected in their original state within 1 min without the need for tedious sample preparation processes. When we use conventional liquid nuclear magnetic resonance (NMR) method to study these systems, the spectral information could not be retrieved owing to the intrinsic inhomogeneous magnetic fields caused by sample inhomogeneity. In addition, the possibility for UF‐iMQC‐based quantifications is shown. The examples presented in this paper demonstrate the potential of UF iMQC NMR for food safety inspection, for quality testing of daily‐life supplies, or in assisting medical diagnosis. Ultrafast high‐resolution spectroscopy based on intermolecular multiple‐quantum coherence is applied for the direct analysis of molecular‐mobility‐restricted samples that are not suitable for magic‐angle spinning, such as a jelly. Through this method, severe signal overlaps (a) have been improved greatly (b), with resolution comparable to a diluted homogenate sample (c).