Today, smart indicators especially based on pigments and natural biopolymers have developed significantly in laboratory and industrial scale. In addition to tracking the freshness and spoilage of the product, these intelligent systems inform the consumer about the quality of the packaged product without opening the package. On the other hand, they reduce food waste and minimize food poisoning. In this study, two halochromic smart indicators were constructed by encapsulating saffron petal and barberry anthocyanins in gelatin/chitin nanofiber films for indication of the freshness/spoilage of fish fillets. Insights into the molecular, structural, and optical properties of these indicators were obtained using X-ray diffraction, scanning electron microscopy, and infrared spectroscopy, and colorimetry analyses. The results showed that the indicators had smooth surfaces and that the pigments were evenly distributed throughout the biopolymer network. The barberry and saffron anthocyanin solutions underwent color changes from reddish to yellow for barberry and reddish to pink to violet to greenish and yellow for saffron anthocyanin after being exposed to different pH values (1–14). The change in appearance of halochromic indicators was quantified by measuring their color coordinates (L*, a*, b*). When applied for estimating fish spoilage, the color of the G/ChNF/BA and G/ChNF/SPA indicators turned from pink to yellow and from violet to green, respectively. After 3 days of storage, the pH and total volatile basic nitrogen of fish fillets reached 8.0 and 49.06 mg N/100 g, respectively. Therefore, a direct relationship between the increase in pH values, the increase in volatile nitrogen bases content, and the changes in the color of the smart indicator applied to monitor the fish was observed. The simulation tests showed that pH-responsive smart indicators can reveal visually fish fillets freshness in real time prior to the point of consumption.