The unique chia–barley composites contain omega-3 polyunsaturated fatty acids (ω-3 PUFAs) from chia and high β-glucan content from barley that are well known for lowering blood cholesterol and preventing coronary heart disease. The pasting and rheological properties of chia and barley composites were characterised using Rapid Visco Analyser followed by an advanced rheometer. Shear-thinning properties were observed for all the composites. The pasting and rheological properties of the products were not greatly influenced by 10% or 20% ground chia replacements but showed differences at the 50% replacement level. The results suggested that the elastic properties of chia–barley composites 1:1 with chia were improved by the chia component. Also, the chia–barley composites gave improved water-holding capacities, particularly at the 50% level. Whole chia seeds are not easily utilised because of their hard coat. These fine particle composites should be helpful for preparing functional food products having enhanced health benefits.