Short answer: radiation poisoning is death to a thousand cuts
Long answer:
Your cells have DNA, which is used as instructions to build and maintain everything in your body. The DNA is copied between cells when they divide, so while a few mutations (errors during copying) won’t likely do much, a lot will.
A large amount of strong radiation (ionizing for example) breaks the bonds in the DNA on a mass scale, which makes some instructions broken or missing. This is like normal mutation, but rapidly sped up all across the body
These rapid mutations cause cells to stop working, leading to an increase of dead cells and lesser efficiency of organs. It also increases the chance of cancer a lot.
Usually what happens during a nuclear fallout, is a long exposure to an increased dose. Radioactive dust is in the air, water is radioactive. All this contributes to the dose which leads to all the above.
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