How do you modify the web.config appSettings at runtime?

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You need to use WebConfigurationManager.OpenWebConfiguration():
For Example:

Dim myConfiguration As Configuration = System.Web.Configuration.WebConfigurationManager.OpenWebConfiguration("~")
myConfiguration.ConnectionStrings.ConnectionStrings("myDatabaseName").ConnectionString = txtConnectionString.Text
myConfiguration.AppSettings.Settings.Item("myKey").Value = txtmyKey.Text
myConfiguration.Save()

I think you might also need to set AllowLocation in machine.config. This is a boolean value that indicates whether individual pages can be configured using the element. If the “allowLocation” is false, it cannot be configured in individual elements.

Finally, it makes a difference if you run your application in IIS and run your test sample from Visual Studio. The ASP.NET process identity is the IIS account, ASPNET or NETWORK SERVICES (depending on IIS version).

Might need to grant ASPNET or NETWORK SERVICES Modify access on the folder where web.config resides.

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