Alcogel has been increasingly applied in foods, cosmetics, and pharmaceutical industries. However, their application is limited by the lack of efficient biomacromolecule-based gelators. Herein, we present our discovery of secalin, a prolamin from rye, combined with konjac glucomannan (KGM) as novel food-grade gelators. Secalin-KGM (SK) alcogels could be prepared by directly cooling down their alcoholic solution, resulting in a thermo-induced sol-gel transition. SK gels (5 w/v % in 50 v/v % ethanol solution) exhibited diverse microstructural features and tunable mechanical properties that could be adjusted by varying the ratio of secalin to KGM. Microscopic images showed that when blended at a certain ratio, a homogeneous porous network is formed due to strong intermolecular interactions. Moreover, the SK gels exhibited a great ability to controllably release curcumin under simulated gastrointestinal tract conditions. The findings provide a novel plant protein-polysaccharide system to develop alcogels with tunable gelling properties and digestibility for functional food and drug delivery applications.