This study explores the combined effects of fuel composition and injection angle on the combustion behavior of an NH3/H2/N2 jet in an air crossflow by means of high-fidelity Large Eddy Simulations (LESs). Four distinct fuel mixtures derived from ammonia partial decomposition, with hydrogen concentrations ranging from 15% to 60% by volume, are injected at angles of 90° and 75° relative to the crossflow, and at operating conditions frequently encountered in micro-gas turbines. The influence of strain on peak flame temperature and NO formation in non-premixed, counter-flow laminar flames is first examined. Then, the instantaneous flow features of each configuration are analyzed focusing on key turbulent structures, and time-averaged spatial distributions of temperature and NO in the reacting region are provided. In addition, statistical analysis on the formation pathways of NO and H2 is performed, revealing unexpected trends: in particular, the lowest hydrogen content flame yields higher temperatures and NO production due to the enhancement of the ammonia-to-hydrogen conversion chemical mechanism, thus promoting flame stability. As the hydrogen concentration increases, this conversion decreases, leading to lower NO emissions and unburned fuel, particularly at the 75° injection angle. Flames with a 90° injection angle exhibit a more pronounced high-temperature recirculation zone, further driving NO production compared with the 75° cases. These findings provide valuable insights into optimizing ammonia–hydrogen fuel blends for high-efficiency, low-emission combustion in gas turbines and other applications, highlighting the need for a careful balance between fuel composition and injection angle.