Novel 5-substituted pyrido[3″,4″:4′,5′]pyrrolo[3′,2′:4,5]imidazo[1,2-a]pyrazine compounds, a method of synthesizing said compounds, a pharmaceutical composition comprising said compounds and a suitable carrier, and a method of using the compounds. The 5-substituted pyrido[3″,4″:4′,5′]pyrrolo[3′,2′:4,5]imidazo[1,2-a]pyrazine compounds, identified as CK2 inhibitors, are useful as anticancer and/or antitumor agents, and as agents for treating other kinase-associated conditions including inflammation, pain, and certain immunological disorders, and other types of diseases such as diabetes, viral infection, neurodegenerative diseases.