Anything is possible but that's not an answer - firstly have you done this since your last post as if you have I'd love to know if you have some sample source that feeds an editable datagrid in asp.net ;-)
If not then to begin with you need to add a reference in the project to the MS Outlook 9 Library - once that's in then it depends what you want to do but the essence of what you want to achieve will be no different to previous examples before .net using CDO, Outlook and ADO.
I'm curious to know what is the most 'elegant' approach to rendering an editable grid - is it wise to stay away from datasets? Probably if the contact folder is large, anyhow I'm busy figuring this one out so if you have been down the route already please let me know!!
Rgds.,
Ed