Actually this is a trap question: it sounds easy but it is not (+1). The short answer to your question is you can't.
I will give an example. Imagine you have 3 Gaussian variables $X_1, X_2$ and $X_3$. You want the correlation between $X_1$ and $X_2$ to be 0, and all correlations with $X_3$ to be 1. This is obviously impossible because $X_1 = X_3$ and $X_3 = X_1$ says that $X_1 = X_2$ (up to shifting and scaling), which contrasts with the assumption that they are independent!
You would have the same situation if you replace 0 by "close to 0" and 1 by "close to 1" in the previous example. The issue here is that not every matrix is a correlation matrix. The requirement for being a correlation matrix is to be symmetric and positive definite.
You cannot choose arbitrary correlation values, but you can check whether they define a valid correlation matrix. Say that you have a symmetric square matrix mat
with required correlation coefficients. You can test that it is positive definite as shown below.
all(eigen(mat)$values >= 0)
For symmetric real matrices, positive definite is equivalent to having all eigenvalues positive.