The techniques of random matrices have played an important role in many machine learning models. In this letter, we present a new method to study the tail inequalities for sums of random matrices. Different from other work (Ahlswede & Winter, 2002 ; Tropp, 2012 ; Hsu, Kakade, & Zhang, 2012 ), our tail results are based on the largest singular value (LSV) and independent of the matrix dimension. Since the LSV operation and the expectation are noncommutative, we introduce a diagonalization method to convert the LSV operation into the trace operation of an infinitely dimensional diagonal matrix. In this way, we obtain another version of Laplace-transform bounds and then achieve the LSV-based tail inequalities for sums of random matrices.