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Let t be a regular operator between Hilbert C*-modules and $t^{†}$ be its Moore-Penrose inverse. We investigate the Moore-Penrose invertibility of the Gram operator t*t. More precisely, we study some conditions ensuring that $t^{†}={(t*t)}^{†}t*=t*{(tt*)}^{†}$ and ${(t*t)}^{†}=t^{†}t{*}^{†}$. As an application, we get some results for densely defined closed operators on Hilbert C*-modules over C*-algebras of compact operators.