Creating layers in foods is a culinary technique commonly used to diversify sensory experiences, but it has not been reported scientifically on its effect on hedonic and appetitive responses. This study aimed to investigate the use of dynamic sensory contrasts in layered foods to stimulate liking and appetite, using lemon mousse as a model. A sensory panel evaluated the perceived sour taste intensity of lemon mousses acidified by various amounts of citric acid. Bilayer lemon mousses with unequal distribution of citric acid across the layers to deliver higher levels of intraoral sensory contrast were developed and evaluated. A consumer panel evaluated the liking and desire to eat lemon mousses (n = 66), and a selection of samples was further investigated in an ad libitum food intake setting (n = 30). In the consumer study, bilayer lemon mousses with a layer of low acidity (0.35% citric acid w/w) on top and higher acidity (1.58 or 2.8% citric acid w/w) at the bottom showed consistently higher liking and desire scores than their corresponding counterparts with identical acid levels equally distributed in a monolayer. In the ad libitum setting, the bilayer mousse (top: 0.35; bottom: 1.58% citric acid w/w) had a significant 13% increase in intake compared to its monolayer counterpart. Modulating sensory properties across food layers with different configurations and layer compositions can be further explored as a tool to design appetizing foods for consumers at risk of undernutrition.