Let $Γ=(K_{n},H^-)$ be a signed complete graph whose negative edges induce a subgraph $H$. The index of $Γ$ is the largest eigenvalue of its adjacency matrix. In this paper we study the index of $Γ$ when $H$ is a unicyclic graph. We show that among all signed complete graphs of order $n>5$ whose negative edges induce a unicyclic graph of order $k$ and maximizes the index, the negative edges induce a triangle with all remaining vertices being pendant at the same vertex of the triangle.