Metal hydrides are an interesting group of chemical compounds, able to store hydrogen in a reversible, compact and safe manner. Among them, A2B7-type intermetallic alloys based on La-Mg-Ni have attracted particular attention due to their high electrochemical hydrogen storage capacity (∼400 mAh/g) and extended cycle life. However, the presence of Mg makes their synthesis via conventional metallurgical routes challenging. Replacing Mg with Y is a viable approach. Herein, we present a systematic study for a series of compounds with a nominal composition of La2-xYxNi6.50Mn0.33Al0.17, x = 0.33, 0.67, 1.00, 1.33, 1.67, focusing on the relationship between the material structural properties and hydrogen sorption performances. The results show that while the hydrogen-induced phase amorphization occurs in the Y-poor samples (x < 1.00) already during the first hydrogen absorption, a higher Y content helps to maintain the material crystallinity during the hydrogenation cycles and increases its H-storage capacity (1.37 wt.% for x = 1.00 vs. 1.60 wt.% for x = 1.67 at 50 °C). Thermal conductivity experiments on the studied compositions indicate the importance of thermal transfer between powder individual particles and/or a measuring instrument.