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I have receive various question about this issue, and I was going to create a tutorial, but I found a great tutorial at Pixel 77. This article is credited to DOINK the author of Pixel 77. He has an amazing site.
So you’ve acquired an impressive collection of vectors and you want to be able to use them asPhotoshop brushes, right ? Well, you can easily transform them into brushes in just a few seconds and I’m here to show you how to do it.

STEP 1

Open your .EPS file in Illustrator and turn all the vector shapes’ color into pure black (#000000). If you vector has more colors, use the Magic Wand (Y) to select each color and hit Delete, leaving only the outline.
(to set Tolerance to “0″, hit Enter after you select the Magic Wand Tool (Y))
1 How to convert vector shapes into Photoshop brushes

STEP 2

Open Photoshop,go to File > New… and create a new document of 2500 x 2500 px in RGB color mode, with the “Background setting set to “White”. (2500 px  is the maximum size for the brushes).[/cleeng_content]
2 How to convert vector shapes into Photoshop brushes

STEP 3

Go back to Illustrator, grab the Selection Tool (V), select a vector shape and copy it (CTRL+C).
3 How to convert vector shapes into Photoshop brushes

STEP 4

Go back to Photoshop and paste it in (CTRL+V). When prompted to select the paste type, check “Smart Object” and hit OK.
4 How to convert vector shapes into Photoshop brushes

STEP 5

Now you’re in Free Transform mode. Resize it to fit the entire document, either on width or height, depends which one is larger. Hit Enter to exit Free Transform mode.
5 How to convert vector shapes into Photoshop brushes

STEP 6

Go to Edit > Define Brush Preset…, name your brush and hit OK. Repeat for the other vector shapes.
6 How to convert vector shapes into Photoshop brushes

STEP 7

To save your brushes, open the Brushes palette (F5) and click the small arrow in the top right corner of the window. Select “Preset Manager”. Here, you can delete any extra brushes, load others or rename the brushes.
Hit OK when you’re done cleaning them up.
7 How to convert vector shapes into Photoshop brushes

7.1 How to convert vector shapes into Photoshop brushes

STEP 8

In the same menu as STEP 7, select “Save brushes…”. Name your set, set its location and hit OK.
8 How to convert vector shapes into Photoshop brushes

DONE!

HOW IT WORKS:

When you define a brush preset, Photoshop only sees you image in grayscale and uses the gray tones to set the opacity of the brush. That’s why you need to set the vectors to pure black and the background color to white.

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