I am trying to do a very strange match up between variables in a loop, may i have help?

It's a bit ambiguous what you want, but here's a few options:

local sf = script.Parent.Parent.Parent.ScrollingFrame
--Get children from firstValue to secondValue
local newCounter
local imageButtons = {}
for _, v in ipairs(sf:GetChildren()) do
    newCounter = v:FindFirstChild("NewCounter")
    if newCounter and newCounter.Value >= firstValue and newCounter.Value <= secondValue then
        table.insert(imageButtons, v)
    end
end
--If you have named each ImageButton in a formulaic way, ex "Image1", "Image2", etc, you can just do this:
local imageButtons = {}
for i = firstValue, secondValue do
    table.insert(imageButtons, sf["Image" .. i]) -- assumes that the ImageButton will always exist
end
--If secondValue is always 1 greater than firstValue and you have "Image1", "Image2", etc:
local firstImage = sf["Image" .. firstValue]
local secondImage = sf["Image" .. secondValue]

--Say you don't have them named in any special way and you want to iterate over all pairs (ex 1,2 followed by 3,4 etc) so that you can apply your Position command:
--First, get all the image buttons into a dictionary/array where the key is newCounter.Value and the value is the image button
local imageButtons = {}
local ch = sf:GetChildren()
local newCounter
local max = 0 -- if you can guarantee that there won't be holes (ex you'll never have "1, 2, 5, 6" without a 3 or 4 anywhere), you don't need max and you can just use #imageButtons instead
for i = 1, #ch do
    newCounter = ch[i]:FindFirstChild("NewCounter")
    if newCounter then
        imageButtons[newCounter.Value] = ch[i]
        if newCounter.Value > max then
            max = newCounter.Value
        end
    end
end
--Now you can iterate over them easily:
for i = 1, max, 2 do
    imageButtons[i].Position = imageButtons[i + 1].Position
end