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The two words mean approximately the same thing but I find that there is a nuance I'm missing in terms of the appropriate context to use one or the other. How should I think about the difference between these two?

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+1, I've also found myself wondering this. Since I don't know the answer I'll just make a comment: Oxford Chinese Dictionary states 确定 is a verb or an adjective, whereas 决定 is a verb or a noun, which at the least means usage is different. – Ming May 9 '14 at 1:53
up vote 10 down vote accepted

确定 means 'be sure' or 'comfirm'/'be confirmed'. 我确定他会回来的.(I'm sure he will be back.)

决定 (v) means 'decide to do'. 我决定做...(I decide to do something...)

决定 (n) means 'decision'. 我终于做出了决定.(Finally, I made my decision.)

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Don't know if this helps - but I think it's useful: 确定, like Soony said, means "to be sure" : so like in English when we want to say "are you sure?!" - in Chinese you can just say "确定吗?" .... but you could never say "决定吗?" if anything you could say "决定了吗?" which would just mean "have you decided?", "have you made a decision?" or "have you made a choice?" ... hope that clears things up a bit – user3306356 May 9 '14 at 3:20
@user3306356 does that make 确定 like 肯定? – Ming May 9 '14 at 5:28
'我确定答案是B' has the same meaning as '我肯定答案是B'. Both of the two sentences mean 'I'm sure the answer is B'. But '肯定' also has a meaning of 'must be'. '这车肯定出故障了'(There must be something wrong with the car.), where you can't use '确定'. It has to be 'SOMEONE 肯定...'. – Soony May 9 '14 at 5:45
@Soony I was following you up until "It has to be 'SOMEONE 肯定...'" because your example used '这车' rather than a someone? – Ming May 9 '14 at 7:31
Ah, my mistake. Obviously I meant 'SOMETHING 肯定 ...'. People use this to state the their conclusion/judgement. – Soony May 9 '14 at 7:57

确定 means sure that / sure to do something.

(我确定他在中午之前一定能把那碗饭吃完。)--> I am sure that he will be able to finish eating that plate of rice.

决定(N) means decision.

(二十分钟后,他终于做出了决定。)--> 20 minutes later, he finally made his decision.

决定(V) means decide to do something.

(我决定吃饭。)--> I decided to eat rice.

Hope this helped. (:

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确定=i am sure that 决定=i decide to do sth

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Sorry this is wrong. Avery's referring to the verb usage of 确定, as in, 'to confirm'. – deutschZuid May 12 '14 at 3:01

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