Novel pyrido[4′,3′:4,5]pyrrolo[3,2-c][1,7]naphthyridin-10-one compounds, a method of synthesizing these compounds, a pharmaceutical composition comprising these compounds and a suitable carrier, and a method of using the compounds. The pyrido[4′,3′:4,5]pyrrolo[3,2-c][1,7]naphthyridin-10-one 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.