The place to start is ~/App_MasterPages/Sugar/DefaultView.master. There is a lot that you can do by changing the master page and the theme files.
Can you be more specific as to what you want to do?
Thanks for your quick reply.
Basically, we would like to re-brand the look of the CRM to match our company's website. Meaning I want to completely change the layout, not just colours and images.
You have the source, so you can do anything you want to the UI. The question you will want to ask yourself is how much do you want to leverage future releases of SplendidCRM. If you are not concerned about applying updates with the least amount of effort, then you are free to redesign the entire application. If you do want to take advantage of bug fixes and new features, then you will likely want to leave the core code unchanged.
The core code is typically located in the user controls EditView, DetailView and ListView. If you are able to leave these files unmodified, then you will be in great shape when applying updates. If you need to make dramatic changes to the EditView, DetailView or ListView, then it is possible to change the core objects that render these views. The place to look is ~/_code/SplendidDynamic.cs and ~/_code/SplendidGrid.cs. These are very complex files, so make sure you know what you are doing if you decided to modify them.