OK, so before I'm crucified for such a title, let me state up front that I love the Brain and have been using it off/on for several years now (along with following the forums).  However, even after watching nearly every new instructional vid that comes out, I still feel that I'm not using my brain nearly as efficiently as I could be.  I have about 667 thoughts in my largest brain but most of the thoughts are parent/child with very few jump-thoughts.  In the past, I've tried repeatedly different techniques that people described here in the forums but with limited success.  I use the Brain mostly for work and my productivity tools include: outlook 2010, onenote, toodledoo (for gtd) and the Brain.  Here's my basic normal routine:
1. outlook 2010 - mail/calendar
2. onenote 2010 - meeting & note capture
3. explorer - document repository (has powerful search capabilities so finding things is not that difficult usually)
4. toodledoo - using a form of GTD I add every action item and move each along the process
5. chrome - web browsing & favorites storage
6. brain - passwords, teleconference info, some documents stored

Out of these tools, the Brain is used the least and I want to be able to use it more but not just as a glitzy toy but as a true tool that duplicates the function of the other tools.  So, having said all that, I guess my question is, how would anyone suggest making this tool as invaluable as I know it should be BUT not by spending a ton of precious time and actually getting the productivity boost that I think I'm missing out on?? Maybe I just haven't had the lightbulb go off in my head yet but I'd love to hear some comments & suggestions.  Thanks in advance! 
Only 667 thoughts will not give you the full benefit of TB. The more you put into it the more useful it gets. Only then you can start to make links and add metadata to it. So with anything you do, read, see, heard of, whatever, put into your brain! One big brain works the best for must people so this is how you can get it to start working for you.

For starters, move your web favourites and bookmarks into TB. I've done this 10 years ago (or whatever it was) and never have needed to use the bookmark facility in whatever browser I use or used. Beside, this is a good starting point as your favourites are quite likely to be the things you are interested and work with.

TB is also excellent as a document repository I think. You can seamlessly link it with the project the document belongs and any other associations you have with.

So in short, stop using all the other tools (if possible of course) and move everything into TB.
PB user since 1998

Mind over matter?
I don't mind and it doesn't matter.
TB Pro on Win10.1 Pro 64bit JVM 1.8.0-112
Thanks Steeph for the great reply.  Bottom line is I can probably do most of what I do with the other tools using just TheBrain so I'll try out your suggestions and see how it goes. 

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