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Sorry, you are missing a hormone.Thyroid hormone levels fluctuate, but if yours has been consistently low, take your medication ie. Synthroid as there is no supplement, vitamin etc that will bring you levels back to normal. I have been on Synthroid since 1992. The only adverse affect can be if you take too much. Have your levels checked a few times a year.
Synthroid is the synthetic thyroid hormone T4. Do not let the word synthetic scare you. After all people take vitamins and mineral supplements and these are all synthetically derived.

Another thought is that, if he has MS and thyroid issues, he might get checked for CCSVI. When the jugular veins are blocked, the flow might be diverted to collaterals such as the thyroid vein, which runs through the thyroid, and might not be suited to handling all that flow.

Welcome.
Your subject title says thyroid cancer. If your husband has indeed cancer of his thyroid gland then it needs surgery to remove some or all of that gland in the neck. They can perhaps destroy the gland with radiation, but he doesn't need to increase it.

If you mean to supplement the gland after surgery, then his doctor with will him on generic levothroxsine, or brand name Synthroid drug for life. He will not be making any of that hormone.

There are other generic name drugs too. If he doesn't have cancer, then iodine is the supplement found in kelp that may help, and many other green moss-like foods that can help, but they usually put a person on a drug, even if synthetic.

Years ago they ground up pig or cow thyroid glands to make thyroid drugs. I am not sure what they do now for the other drugs that are available. If you just want food supplements I could look them up for you.

Let us know what his thyroid medical issue is, okay? Jimmylegs is excellent with food supplements for good health.
CD