I will assume that your amended title is acceptable.

I think you will need to help us understand the math behind what you want to do before we can help you. From what I have gathered in some quick internet searches:

Wikipedia's article talks mostly about using the Cholesky decomposition in solving systems of equations. I cannot readily see how your problem reduces to a "solve a system of equations" kind of problem. If this is how Cholesky's decomposition would apply to your problem, I would probably suggest that you set up your system of equations and then use Excel's built in MINVERSE() function (which uses QR decomposition rather than Cholesky's decomposition) to help solve the system of equations.

If it does not reduce to a system of equations, but the Cholesky decomposition fits into the problem in a different way, generating the Cholesky decomposition should be as "simple" as working through the Gaussian elimination steps to generate the decomposition matrices. These steps can be accomplished in Excel using the MMULT() function.

If the Cholesky decomposition is not an integral part of the solution, I could see using Solver for this sort of thing. Given two data sets, and using the CORREL() function (or whatever function represents your "correlation" score), you could call Solver and tell it to set the CORREL() function cell to a value of -0.05 by changing one or more of the values in the 2nd data set. I expect there are multiple possible solutions to most of these problems. If any solution is acceptable (and you don't need to find a specific solution), this might be the easiest to implement in Excel.