Chrysanthemum is one of the most attractive flowering plants widely grown commercially worldwide. Having a good source of organic fertilizers plays an important role in meeting the increasing demand for these plants, which requires high-quality flowers and a high survival time for the longest period. The effect of nitrogen (N) coupled with spent coffee ground (SCG) at various levels (0.0, 2.5, 5.0, 7.5, 10.0°% w/w) was evaluated on growth performance and chemical components of the Chrysanthemum over two years in a pot scale. Overall, total dry matter (TDM) was significantly enhanced with N+ by 125 and 97°% over N− in the first and second years, respectively. SCG also enhanced TDM up to the highest level of application in the range of 27–98°% and 18–81°% over SCG (0.0°%) in the same years, respectively. The interaction effect between N and SCG was perfect on TDM, flower number, and flower dry weight. Similarly, total antioxidant activities when N and SCG were coupled together gave respective increments ranging from 11.8 to 45.9 U/g DW and from 2.1 to 15.9 U/g DW compared to N alone (5.8 and 0.9 U/g DW) in both leaves and flowers, respectively. Extracts of plant treated with N and 10°% SCG exhibited a higher content of rosmarinic, caffeic, chlorogenic, vanillic acids, and rutin in the leaves. SCG as a natural organic source is easy to obtain and is a practical and cost-effective solution to plant nutrition, which can be valuable for ornamental plants, especially when combined with nitrogen.