I'm using 6.1.5 on two instances ... on one instance, I can add roles without a problem (User Accounts >> Edit User Accounts >> Manage Roles for User) ... in the other instance, I cannot add a role to a user ... when I click 'Add Role to User' it looks like the Ajax process begins, but then the role is not added ... the exception to this is the 'Administrators' role ... I can add that role to any user in both instances.

In Security Roles >> Edit Security Roles >> Manage Users in Role I can add any user to the any of the roles.

So, the problem is adding roles to a user.

There is no exception in the Event Viewer.

you could try enabling log4net to All (http://www.dotnetnuke.com/Resources/Wiki/Page/log4net-In-DotNetNuke.aspx) to see if that captures anything, but if not then perhaps check if there is a javascript error happening (see the F12 tools or firebug if using firefox) as perhaps something skin related is caused a script exception

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