The set of unicyclic graphs with vertices and diameter is denoted by . For , let be the graph obtained from path by adding pendant edges at , and be the graph obtained from by joining and a pendant neighbor of . In this paper, we determine all unicyclic graphs in whose largest Laplacian eigenvalue is greater than . For and , we prove further that the largest Laplacian eigenvalue , and conjecture that is the unique graph which has the greatest value of the greatest Laplacian eigenvalue in . We also prove that the conjecture is true for .