Indole is a chemical from the decomposition of shrimp and is used extensively to indicate seafood freshness. US Food and Drug Administration (FDA) sets its concentration of <25 μg/100 g shrimp as the threshold for Class I (fresh shrimp). A novel optical probe is reported to quantitatively analyze trace indole in shrimp, including the Class I threshold concentration. Based on an Ehrlich-type reaction, visible spectroscopic analysis of indole in petroleum ether gives a limit of detection (LoD) and quantification (LoQ) of 0.05 and 0.16 μg mL−1, respectively. For 25 μg indole/100 g shrimp extracted into petroleum ether, the probe successfully detects it and the color change is visible to the naked eye. Analysis of the probe response by a visible spectrometer leads to quantification of ≤25 μg indole/100 g shrimp, when recovery is accounted for. When a handheld colorimeter, based on the CIELAB color space, and a smartphone with Bluetooth connectivity are used, the probe demonstrates similar sensitivity for indole in shrimp. The current probe is made of 4-(dimethylamino)benzaldehyde (DMAB) and catalyst p-toluenesulfonic acid (PTSA) in thin films. Indole in shrimp samples after extraction reacts with DMAB to give red β-bis(indolyl)methane.