This study showed that the incorporation of whole chia flour (WCF) resulted in a nutritionally enhanced pound cake, mainly in relation to the omega-3 α-linolenic acid content and omega-6/omega-3 ratio. It is possible to incorporate WCF into pound cake formulations and obtain a product with good technological and sensory performances. The presence of hydrogenated vegetable fat (HVF) helps to minimize the adverse effects of WCF on the specific volume and firmness of the cakes. The best technological results were obtained for cakes produced with up to 15 g WCF/100 g flour mixture and from 16 to 20 g HVF/100 g flour mixture.