Your terminology is a little confusing: there is no such thing as "Windows XP .NET 4.0", but it sounds like you want to use .NET 4.0 on Windows XP. That would be OK. Note that your POS must be running Windows XP SP3. Note that .NET 4.5 and above are not supported in Windows XP. Your new DLLs must be compiled under .NET 4.0 or earlier. There are special complications if your POS software already uses .NET for anything else. I'll assume here that you are using .NET 4.0 and that the POS doesn't otherwise depend on .NET.
You do need to install on the POS machines an appropriate version of the .NET runtime (the version under which your DLL has been compiled is the best choice). But after that - yes, of course RegAsm will allow you to register a COM DLL (not RegSvr32 however; RegSvr32 doesn't know how to register a .NET DLL). As I mentioned in a my previous comment, the details in the registry will necessarily be different from the details for the VB6 DLL.
The installers for the different supported .NET runtimes are available from Microsoft. There are two options:
The ".NET 4.0 Client Profile installer" is currently available here:
http://www.microsoft.com/en-us/download/details.aspx?id=24872
The "Full .NET installer" is currently available here:
http://www.microsoft.com/en-us/download/details.aspx?id=17718
If you can help it, you want to compile your DLL using the ".NET 4.0 Client Profile" option, which is a subset of the whole runtime with only the most commonly used features. The Client Profile is significantly smaller. You will know immediately if your application is compatible with the Client Profile simply by trying to compile it with that option. If you are using something that is not included in the Client Profile, your DLL will fail to compile. In that case, try first to see if you can accomplish the same functionality without using the non-client-profile feature. If you can't, then use the full runtime.
Now the hard part: you don't specify if your DLL exposes a bunch of custom interfaces, whether it only consumes interfaces declared by the application, or a combination of both. You also don't specify how the POS software knows about your DLL and whether it uses Automation (IDispatch) like VBScript would or "custom" interfaces, and you don't say who declares the interfaces. Setting up the appropriate interfaces in C#/VB.NET can be a tricky problem because VB6 doesn't exactly make it easy to look at the details.
You can pull the most critical information from the existing DLL by registering it and looking at the resulting classes via the "OLE View" tool. The rest of the details will depend on how the main POS application uses your DLL. The full details of what to do can be complex and are well outside of the scope of any one single answer in Stack Overflow.