First, reliability estimates in the 0.6 - 0.7 range are not great, but they're not completely awful.
There are a lot of things that you could do. It's not as easy to say what you should do.
You got low reliability. That's not great for your research. Your may not be great measures. But they still might be. One thing you can do in your write up is say "Reliability was low, so perhaps results are less trustworthy". But there are many possible reasons for this. You could investigate these reasons.
Alpha is a function of variance - if you have low variance, you will have low reliability - that is, everyone giving very similar answers. Say you have a 5 point scale about how much you like cats. And you give it out at a cat fancier's meeting, everyone will answer with 4 and 5. Your reliability will be low. Combine that with data you collect at a dog fancier's meeting, the reliability will increase, because the variance will increase.
Perhaps it's particular items. You could examine individual items, using things like the item-total correlation. Maybe the scales improve if you remove an item that didn't work well. (Example: To an American, the word 'touchy' means sensitive, easily offended. To a British person, it might mean 'tactile' - likes touching people. If you keep the item 'touch' in a measure of sensitivity, the reliability might be low in a British sample.
You could do factor analysis to investigate the underlying structure of the scales.
Alpha is an estimate of reliability, but to interpret it as reliability makes the assumption that there is an underlying latent variable which is the cause of the responses to the items. You think there is a variable called happiness, and this causes many behaviors - happy people smile more, sleep more, laugh more. Or is happiness a function of things that happen to me: I get enough sleep, I'm paid enough, I have friends, I have a supportive family - perhaps these things cause happiness. If the latter is the case, alpha is not a good estimate of reliability. What is the relationship in your data?
How big was the sample? You could investigate the confidence intervals of alpha.
You could investigate whether there are subgroups for whom the TSI has higher alpha. Perhaps it's not relevant to some people, so they're not able to answer. If I ask people to complete my "CrossValidated Style Inventory" most people don't have a CrossValidated style, so they can't give sensible answers that make sense. But heavy users (and answerers) of CrossValidated could be measured on many questions (answer length, use of equations, answer frequency, critical style, etc).