You don't explain what the role of .NET would be in your scenario. You can indeed call many C libraries directly from VBA using 'Declare Function'.
If you find .NET useful, and want to call your .NET library functions as user-defined functions (UDFs) from Excel, you can use Excel-DNA. It gives you an .xll add-in library that integrates your .NET library into Excel. You'd still have to open the .xll add-in somehow - either by File -> Open, by adding it as an Excel add-in, or automatically from some VBA in your workbook. But it needs no other registration.
From the .NET library you can call the C .dll functions using P/Invoke, add categories, function and argument descriptions to integrate into the function wizard etc.
(Disclaimer: I'm the developer of Excel-DNA.)
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