The three Germans behind Ballonmoleküle give lots of information on how to make molecule models out of long balloons, and explain why you would want to use balloons:
The balloons automatically adjust every angle in a way that an atom according to modern atom models does, too. When three balloons meet at one knot (at the atomic nucleus so to speak), they act just like a sp2-hybrid atom which means they form a planary system. When four balloons meet, they form a tetrahedral. You only have to keep in mind to build some free electron pairs as well. If you do this for example for water, there will be a smaller angle than for a tetrahedral, since there are six balloons that meet in one knot (two compounds for the hydrogen atom and two each for one free electron pair).
They even get a shout-out from Francis Crick: "It's really remarkable how you have been able to show the key elements of the double helix with balloons."
Next time you're at a fair, ask the clown with the balloons to make you a Cuban cluster
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