This study aimed to develop a high-protein and gluten-free laver chip using air-frying and reaction flavor technologies via response surface methodology (RSM). The optimum processing condition (w/w) was determined with a batter composition of 20% dried laver, 21.3% hair tail surimi, and 58.7% rice flour. Additional ingredients included б-gluconolactone, NaHCO3, soybean oil, corn syrup, table salt, saccharin, and a mixture of distilled water and reaction flavor-inducing solution (RFIS). The laver pellet processed and dried (50 °C, 1–2 h) with air-frying (195 °C, 52.5 s) to process the laver chip. The values of brittleness and puffing ratio of the laver chip were 6.93 ± 0.33 N and 116.19 ± 0.48%, respectively, with an error within 10% of the predicted values of RSM. RFIS was prepared via RSM with the addition of precursor substances (w/v) of methionine 0.54%, threonine 3.30%, glycine 2.40%, glutamic acid 0.90%, and glucose 3% to distilled water and then heating reaction (121 °C, 90 min). The quantitatively descriptive analysis (QDA) of RFIS, baked potato-like and savory odor were 6.00 ± 0.78 and 4.00 ± 0.91, respectively, with an error within 10% of the predicted values. The laver chip exhibited high-protein (24.26 ± 0.10 g%) and low-calorie (371.56 kcal) contents.