While bitcoin-qt is downloading the chain to synchronize with the network, opening the coin control dialog box makes the GUI unresponse with no notification to the user on what is occuring. This is duplicatable behavior for me, and gui lockup time varied from as high as a minute to as low as 8 second. As soon as the blockchain is syncronized, no gui lockup occurs.
Step 1: Open up a Bitcoin Core wallet that is behind on synchronization. Mine was behind about 48 hours, giving me a few minutes to test before synchronization was complete.
Step 2: Go to the Send tab, and in the Coin Control Features box click 'Inputs...'. The app will no become unresponsive for roughly 30 seconds and after some time the coin selection dialog will eventually appear.
Step 3: Try to reproduce after blockchain is fully syncronized. Notice that no more delay is occurring.
Verified on Bitcoin Core version v0.10.1 (64-bit) linux.
Theory: Verifying incoming blocks is taking a lot of CPU. Pulling up the Coin Selection dialog may also take some CPU to construct the Tree of Transactions. (My wallet was very small with only a few entries, but non the less my gui was still locking up.) Perhaps the app can prioritize building the Coin Selection window for the user over any background processes that are verifying blocks. The Background block verifying should be a lower priority background thread, though i admit I know little about how threading works or if this is what is actually causing the issue.